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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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43 records · Page 3

Probing Clustering Dynamics between Silicon and PAA or LiPAA Slurries under Processing Conditions

This work explores the complex interplay between slurry aggregation, agglomeration, and conformation (i.e., shape) of poly(acrylic acid) (PAA)- and lithiated PAA-based silicon slurries as a function of the shear rate and the resulting slurry homogeneity. These values were measured by small-angle neutron scattering (SANS) and rheology-coupled ultra-SANS at conditions relevant to battery electrode casting. Different binder solution preparation methods, either a ball milling (BM) process or a planetary centrifugal mixing (PCM) process, dramatically modify the resulting polymer dynamics and organization around a silicon material. This is due to the different energy profiles of mixing where the more violent and higher energy PCM causes extensive breakdown and reformation of the binder, which is now likely in a branched conformation, while the lower energy BM results in simply lower-molecular weight linear polymers. In conclusion, the breakdown and reorganization of the polymer structure affect silicon slurry homogeneity, which affects subsequent electrode architecture.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structure and dynamics of small polyimide oligomers with silicon as a function of aging

The effect of UV curing and shearing on the structure and behavior of a polyimide (PI) binder as it disperses silicon particles in a battery electrode slurry was investigated. PI dispersant effectiveness increases with UV curing time, which controls the overall binder molecular weight. Here, the shear force during electrode casting causes higher molecular weight PI to agglomerate, resulting in battery anodes with poorly dispersed Si particles that do not cycle well. It is hypothesized that when PI binder is added above a critical amount, it conformally coats the silicon particles and greatly impedes Li ion transport. There is an “interzonal region” for binder loading where it disperses silicon well and provides a coverage that facilitates Li transport through the anode material and into the silicon particles. These results have implications in ensuring reproducible electrode manufacturing and increasing cell performance by optimizing the PI structure and coordination with the silicon precursor.

36 MATERIALS SCIENCE↗

Development of a Novel Magnesium Alloy for Thixomolding® of Automotive Components (Final Report)

Magnesium (Mg) alloy die-castings are increasingly used in the automobile industry to achieve cost effective mass reduction, especially in systems where multiple components can be integrated into a single thin wall die-casting. However, there are several component quality restrictions in thin-walled Mg die castings, including variability in dimensional accuracy, part-to-part variation in mechanical properties, and porosity in the final part, which has limited the continued growth of die-cast components in the automobile industry. An alternative to die-casting is the process of thixomolding®. While the die-casting process relies on filling a mold at high speeds with the alloy in the completely molten state, the thixomolding® process fills a mold with a thixotropic alloy in a semi-solid slurry state at a temperature between the liquidus and solidus temperatures. Ideally, the material should be ~30–65% solid rather than being completely liquid at the beginning of the injection process. Advantages of the thixomolding® process include a finer grain structure, lower porosity, improved dimensional accuracy, improved part-to part consistency, improved mechanical properties, particularly ductility in the component, the ability to reduce wall thickness for mass savings, and longer tool life due to lower process temperatures. The objective of this collaborative project between Oak Ridge National Laboratory, FCA US LLC, and Leggera Technologies was to develop one or more novel Mg alloys more suitable for thixomolding® automotive structural components than the current die-casting alloys used for this process. The primary interest was to improve ductility while maintaining tensile and fatigue strengths, as these are properties that are critical for use in body and chassis structural applications. Since good corrosion resistance is also desirable for this application, this property was also considered when evaluating promising alloy compositions. An initial evaluation of existing components thixomolded® using AM60 was performed and microstructure, and tensile properties were evaluated for the baseline alloy. Targets were established for ease of processing (characterized by the melting range defined as the difference between the liquidus and the solidus), strength, and ductility. Computational modeling was used to identify promising alloys and selected alloys were cast in laboratory scale heats. Properties measured from laboratory scale heats were used to down-select two alloys for further evaluation and component fabrication. Two alloys were prepared in industrial scale heats, cut into small pieces (chips), and thixomolding® trials were initiated. Trial components were successfully fabricated using one alloy composition, but it was concluded that further refinement of the thixomolding® process parameters are required to successfully fabricate component using second alloy. Microstructure and mechanical properties were evaluated on the material removed from the fabricated component and properties were compared to the baseline alloy. Although mechanical properties of the alloys showed improvement over the baseline alloy, it was determined that modifications to the thixomolding® process would result in better microstructure control with further improvement in properties leading to successful commercialization. A provisional patent application has already been filed on the new alloys developed as part of the project.

36 MATERIALS SCIENCE↗

Scalable Freeze-Tape-Casting Fabrication and Pore Structure Analysis of 3D LLZO Solid-State Electrolytes

Nonflammable solid-state electrolytes can potentially address the reliability and energy density limitations of lithium-ion batteries. Garnet-structured oxides such as Li 7 La 3 Zr 2 O 12 (LLZO) are some of the most promising candidates for solid-state devices. Here, three-dimensional (3D) solid-state LLZO frameworks with low tortuosity pore channels are proposed as scaffolds, into which active materials and other components can be infiltrated to make composite electrodes for solid-state batteries. To make the scaffolds, we employed aqueous freeze tape casting (FTC), a scalable and environmentally friendly method to produce porous LLZO structures. Using synchrotron radiation hard X-ray microcomputed tomography, we confirmed that LLZO films with porosities of up to 75% were successfully fabricated from slurries with a relatively wide concentration range. The acicular pore size and shape at different depths of scaffolds were quantified by fitting the pore shapes with ellipses, determining the long and short axes and their ratios, and investigating the equivalent diameter distribution. The results show that relatively homogeneous pore sizes and shapes were sustained over a long range along the thickness of the scaffold. Additionally, these pores had low tortuosity and the wall thickness distributions were found to be highly homogeneous. These are desirable characteristics for 3D solid electrolytes for composite electrodes, in terms of both the ease of active material infiltration and also minimization of Li diffusion distances in electrodes. The advantages of the FTC scaffolds are demonstrated by the improved conductivity of LLZO scaffolds infiltrated with poly(ethylene oxide)/lithium bis(trifluoromethanesulfonyl)imide (PEO/LITFSI) compared to those of PEO/LiTFSI films alone or composites containing LLZO particles.

36 MATERIALS SCIENCE↗

Roll-to-Roll Advanced Materials Manufacturing DOE Laboratory Collaboration (FY2019 Final Report)

R2R processing is used to manufacture a wide range of products for various applications which span many industrial business sectors. The overall R2R methodology has been in use for decades and this continuous technique traditionally involves deposition of material(s) onto moving webs, carriers or other continuous belt-fed or conveyor-based processes that enable successive steps to build a final version which serves to support the deposited materials. Established methods that typify R2R include tape casting, silk-screen printing, reel-to-reel vacuum deposition/coating and R2R lithography. Products supported by R2R manufacturing include micro-electronics, electro-chromic window films, PVs, fuel cells for energy conversion, battery electrodes for energy storage, and barrier and membrane materials. Due to innovation in materials and process equipment, high-quality yet very low-cost multilayer technologies have the potential to be manufactured on a very cost-competitive basis. To move energy-related products from high-cost niche applications to the commercial sector, a means must be available to enable manufacture of these products in a cost-competitive manner that is affordable. Fortunately, products such as fuel cells, thin- and mid-film PVs, batteries, electrochromic and piezoelectric films, water separation membranes, and other energy saving technologies readily lend themselves to manufacture using R2R approaches. However, more early-stage research is needed to solve the challenge of linking the materials (particles, polymers, solvents, additives) used in ink and slurry formulations, though the ink processing, coating and drying processes, to the ultimate performance of the final R2R product, especially for a process that uses multiple layers of deposition to achieve the end product.

42 ENGINEERING↗

Roll-to-Roll Advanced Materials Manufacturing DOE Laboratory Collaboration (FY2020 Final Report)

R2R processing is used to manufacture a wide range of products for various applications which span many industrial business sectors. The overall R2R methodology has been in use for decades and this continuous technique traditionally involves deposition of material(s) onto moving webs, carriers or other continuous belt-fed or conveyor-based processes that enable successive steps to build a final version which serves to support the deposited materials. Established methods that typify R2R processing include tape casting, silk-screen printing, reel-to-reel vacuum deposition/coating, and R2R lithography. Products supported by R2R manufacturing include micro-electronics, electro-chromic window films, PVs, fuel cells for energy conversion, battery electrodes for energy storage, and barrier and membrane materials. Due to innovation in materials and process equipment, high-quality yet very low-cost multilayer technologies have the potential to be manufactured on a very cost-competitive basis. To move energy-related products from high-cost niche applications to the commercial sector, the means must be available to enable manufacture of these products in a cost-competitive manner that is affordable. Fortunately, products such as fuel cells, thin- and mid-film PVs, batteries, electrochromic and piezoelectric films, water separation membranes, and other energy saving technologies readily lend themselves to manufacture using R2R approaches. However, more early-stage research is needed to solve the challenge of linking the materials (particles, polymers, solvents, additives) used in ink and slurry formulations and the coating and drying processes to the ultimate performance of the final R2R product, especially for a process that uses multiple layers of deposition to achieve the end product. To solve the problems associated with these challenges, the R2R Collaboration is executing a research program with outcomes that will ultimately link modeling, processing, metrology and defect detection tools, thereby directly relating the properties of constituent particles and processing conditions to the performance of final devices. This collaborative approach was designed to foster identification and development of materials and processes related to R2R for clean-energy materials development. Using computational and experimental capabilities by acknowledged subject matter experts within the supported National Laboratory system, this project leverages the capabilities and expertise at each of five National Laboratories to further the development of multilayer technologies that will enable high-volume, cost-competitive platforms. A typical R2R process has three steps: (1) mixing of particles and various constituents in a slurry, (2) coating of the ink/slurry mixture on a substrate, and (3) drying/curing and processing of the coating. Final performance of devices made via R2R processes is dependent on the active materials (e.g., electrochemical particles in battery or fuel cell electrodes) and the device structure that stems from the governing component interactions within the various steps. However, a fundamental understanding of the underlying mechanisms and phenomena is still lacking, which is why industrial-scale R2R process development and manufacturing is still largely empirical in nature. The FY 2019 through FY 2021 program addresses aspects of the following two targets from the AMO Multi-Year Program Plan: (1) Target 8.1 Develop technologies to reduce the cost per manufactured throughput of continuous R2R manufacturing processes. (A) Increasing throughput of R2R processes by 5 times for batteries (to 50 square feet per minute (50 ft 2 /min)) and capacitors and 10 times for printed electronics and the manufacture of other substrates and MEs used in support of these products. (B) Developing resolution capabilities to enable registration and alignment that will detect, align, and co-deposit multiple layers of coatings and print < 1-micron (1 µm) features using continuous process scalable for commercial production. (C) Developing scalable and reliable R2R processes for solution deposition of ultra-thin (<10 nm) films for active and passive materials. (D) Develop in-line multilayer coating technology on thin films with yields greater than 95%. (2) Target 8.2 Develop in-line instrumentation tools that will evaluate the quality of single and multilayer materials in-process. (A) Developing in-line QC technologies and methodologies for real-time identification of defects and expected product properties “in-use/application” during continuous processing at all size-scales with a focus on the “micro” and “nano” scale traces, lines, and devices, i.e., <1 μm at 300 ft./min for R2R processing in air and <10 nm at 20 ft./min for vacuum (B) Developing technologies to increase the measurement frequency of surface rheology without significant cost increases with a goal of a 10-nanometer in-line profilometry at a production rate of 100,000 square millimeters per minute (100,000 mm 2 /min).

42 ENGINEERING↗

Roll-to-Roll Advanced Materials Manufacturing DOE Laboratory Collaboration - Early Stage R&D: Phase 2 and FY21 (Final Report)

R2R processing is used to manufacture a wide range of products for various applications which span many industrial business sectors. The overall R2R methodology has been in use for decades and this continuous technique traditionally involves deposition of material(s) onto substrates or membranes that are on moving webs, carriers or other continuous belt-fed or conveyor-based processes that enable successive steps to build a final product. Established methods that typify R2R processing include tape casting, silk-screen printing, reel-to-reel vacuum deposition/coating, and R2R lithography. Products supported by R2R manufacturing include micro-electronics, electro-chromic window films, PVs, fuel cells for energy conversion, battery electrodes and electrolytes for energy storage, and barrier and membrane materials for decarbonization and air and water filtration. Due to innovation in materials and process equipment, high-quality yet very low-cost multilayer technologies have the potential to be manufactured on a very cost-competitive basis. To move energy-related products from high-cost niche applications to the commercial sector, the means must be available to enable manufacture of these products in a cost-competitive manner. Fortunately, products such as fuel cells, thin- and mid-film PVs, batteries, electrochromic and piezoelectric films, water separation membranes, and other energy saving technologies readily lend themselves to manufacture using R2R approaches. However, more early-stage research is needed to solve the challenge of linking the materials (particles, polymers, solvents, additives) used in ink and slurry formulations and the coating and heated drying processes to the ultimate performance of the final R2R product, especially for a process that uses multiple layers of deposition to achieve the end product.

36 MATERIALS SCIENCE↗